CN113066901B - Enhanced VO x -Ga 2 O 3 Method for self-powered photoresponse performance of heterojunction - Google Patents
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Abstract
Enhanced VO x ‑Ga 2 O 3 A method of heterojunction self-powered photoresponsive performance, comprising: preparation of VO x ‑Ga 2 O 3 Heterojunction, to the prepared VO x ‑Ga 2 O 3 And carrying out secondary specific atmosphere annealing on the heterojunction to improve the separation capability of electron-hole and the carrier transport capability. The method of the invention can change the contact characteristics and VO at the interface x Valence ratio of V element of material and Ga 2 O 3 The crystal quality of the material effectively promotes VO x ‑Ga 2 O 3 The self-powered photoresponse performance of the heterojunction photoelectric device is improved; the method has the advantages of simple operation, low cost and obvious effect, and is favorable for scientific research reference and industrial production flow.
Description
Technical Field
The invention belongs to the field of semiconductor optoelectronic devices, particularly relates to a self-powered photoresponse performance optimization method of a heterojunction device, and especially relates to a VO (vacuum integrated photovoltaics) enhancement method x -Ga 2 O 3 A method of heterojunction self-powered photoresponsive performance.
Background
The increasing energy demand of human society and the imbalance of the earth's traditional fossil resource supply have become a serious challenge in today's world. In order to solve the problem of insufficient energy supply and promote innovation of energy technology, scientists around the world have gradually developed renewable energy sources including water energy, solar energy, wind energy, tidal energy and the like for nearly half a century. The use of the clean energy relieves the urgency of energy supply to a certain extent and also points out the direction for the use of new energy for human beings. In addition to seeking for the use of natural clean energy, a great part of scientists have sought to create a self-powered system. In the system, the system can generate and store energy by sensing the change of the external environment, and supports the work of the electronic device. Such a self-powered system has independence, sustainability, and wireless modes of operation. The popularization and the application of the energy-saving and energy-saving agent can greatly reduce the consumption and the dependence of human beings on traditional energy sources. As a new development direction and technology in the field of self-powered system research, a self-powered photodetector is a device that can convert an optical signal into an electrical signal without external energy support, and has attracted much attention in recent years because of its important applications in environmental monitoring, optical communication, national defense early warning and imaging technologies. The basic physical mechanisms of a self-powered photodetector are: (1) absorbing incident photons to generate electron-hole pairs; (2) separating the electron-hole pairs under the built-in electric field; (3) The photogenerated carriers are collected by an external circuit to realize the conversion of signal light into electricity. The built-in potential is the source of the separation power for electron-hole pairs, and thus in order to fabricate a self-powered detector, a built-in electric field needs to be created at the photon absorption interface. Common structures used to fabricate self-powered photodetectors are mainly p-n homojunctions, heterojunctions, and schottky junctions.
Gallium oxide (Ga) 2 O 3 ) Since the last 50 s of the century, it has been considered as the most suitable material for solar blind photodetectors because of its ultra-wide band gap of 4.6-5.1 eV. Especially in recent years, based on high quality Ga 2 O 3 Epitaxial material, ga was developed 2 O 3 The self-powered photoelectric detector obtains the responsiveness performance of ampere per watt. However, research based on this field and prototypes prepared are limited to verification of self-powered performance, and how to promote and optimize Ga 2 O 3 The self-powered performance of base photovoltaic devices has not been extensively studied and systematically studied. Li Qing Ga 2 O 3 The influence mechanism and the optimization mechanism of the self-powered photoresponse performance of the base photoelectric device are important links for the future expansion and commercial application of the devices.
Disclosure of Invention
In view of the above, the main objective of the present invention is to provide an enhanced VO x -Ga 2 O 3 Heterojunction self-powered electro-optic loudspeakerMethod for preparing the same and the preparation of the VO x -Ga 2 O 3 A method of heterojunction and an optoelectronic device employing the same, intended to at least partially solve at least one of the above technical problems.
To achieve the above object, as a first aspect of the present invention, there is provided a VO enhancement x -Ga 2 O 3 A method of heterojunction self-powered photo-responsive performance, comprising the steps of:
preparation of VO x -Ga 2 O 3 A heterojunction;
to the prepared VO x -Ga 2 O 3 And carrying out secondary specific atmosphere annealing on the heterojunction to improve the separation capability of electron-hole and the carrier transport capability.
As a second aspect of the invention, there is also provided a VO x -Ga 2 O 3 The preparation method of the heterojunction comprises the following steps:
preparation of VO x -Ga 2 O 3 A heterojunction;
for the prepared VO x -Ga 2 O 3 And carrying out secondary specific atmosphere annealing on the heterojunction to improve the separation capability of electron-hole and the carrier transport capability.
As a third aspect of the present invention, there is also provided VO prepared according to the preparation method as described above x -Ga 2 O 3 A heterojunction.
As a fourth aspect of the present invention, there is also provided a photovoltaic device, wherein the photovoltaic device comprises the VO as described above x -Ga 2 O 3 A heterojunction.
Based on the technical scheme, the method for enhancing self-powered photoresponse performance and the prepared VO x -Ga 2 O 3 Compared with the prior art, the heterojunction, the preparation method thereof and the photoelectric device comprising the heterojunction have at least one of the following beneficial effects:
the invention is to prepare the prepared VO x -Ga 2 O 3 The heterojunction is subjected to a second annealing in a specific atmosphere,changing contact characteristics and VO at an interface x Valence ratio of V element of material and Ga 2 O 3 The crystal quality of the material can improve VO x -Ga 2 O 3 The electron-hole separation capability and the carrier transport capability of the heterojunction realize VO x -Ga 2 O 3 The heterojunction self-powered photoresponse performance is improved;
the invention optimizes the working mechanism of the device on the basis of the working principle of a heterojunction photoelectric device and effectively realizes VO x -Ga 2 O 3 The enhancement of the self-powered light response performance of the heterojunction photoelectric device clears the working principle and the regulation mechanism of the self-powered photoelectric device;
the method has the advantages of simple operation, low cost and obvious effect, and is favorable for scientific research reference and industrial production flow.
Drawings
FIG. 1 shows the initial preparation and secondary annealing treatment of VO in example 1 of the present invention x -Ga 2 O 3 Dark current and photocurrent curves for heterojunction photovoltaic devices;
FIG. 2 shows the initial preparation and secondary annealing treatment of VO in example 1 of the present invention x -Ga 2 O 3 The photoresponse current of the heterojunction photoelectric device changing with the optical switch;
FIG. 3 shows the initial preparation and secondary annealing treatment of VO in example 1 of the present invention x -Ga 2 O 3 A spectral response curve of the heterojunction photovoltaic device;
FIG. 4 shows the initial preparation and secondary annealing treatment of VO in example 1 of the present invention x A current-voltage curve of the material;
FIG. 5 is an initial preparation of VO of example 1 of the present invention x -Ga 2 O 3 A band alignment schematic of the heterojunction;
FIG. 6 shows the VO of the second annealing treatment in example 1 of the present invention x -Ga 2 O 3 Heterojunction energy band alignment schematic.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail with reference to the accompanying drawings in combination with the embodiments.
The present invention is directed to Ga 2 O 3 The self-powered photoresponse performance influence mechanism and regulation mechanism of the base photoelectric device are unclear, and the self-powered photoresponse performance influence mechanism and regulation mechanism are provided by carrying out VO treatment on the base photoelectric device x -Ga 2 O 3 The specific atmosphere annealing treatment of the heterojunction improves the separation capability of electron-hole pairs of a built-in electric field and improves the p-type VO x Hole conductivity of the material and n-type Ga 2 O 3 The electronic conductivity of the material is optimized to optimize the physical mechanism of the photoelectric device, and VO is realized x -Ga 2 O 3 Enhancement of heterojunction self-powered photoresponse performance.
Specifically, the invention discloses a reinforced VO x -Ga 2 O 3 A method of heterojunction self-powered photo-responsive performance, comprising the steps of:
preparation of VO x -Ga 2 O 3 A heterojunction;
to the prepared VO x -Ga 2 O 3 Secondary specific atmosphere annealing is carried out on the heterojunction to improve the separation capability of electron-hole and the carrier transport capability and realize VO x -Ga 2 O 3 And the heterojunction self-powered photoresponse performance is improved.
Wherein, the VO x -Ga 2 O 3 The heterojunction is one of a planar heterojunction and a vertical heterojunction.
VO thus prepared x -Ga 2 O 3 In the heterojunction, ga 2 O 3 Is a film with the thickness of 50-900 nm, VO x Is a thin film with the thickness of 5-200 nm. Further preferably, ga 2 O 3 The thickness of the film is 200-500nm, VO x The thickness of the film is 20-50 nm.
The Ga 2 O 3 The film can be prepared by one or more combined techniques of metal organic chemical vapor deposition, pulsed laser deposition, molecular beam epitaxy or magnetron sputtering.
The VO x The film can pass throughChemical precursor spin coating, pulsed laser deposition or magnetron sputtering.
Wherein the specific atmosphere is formed by one or more of air, oxygen, argon and nitrogen. Preferably, the specific atmosphere is argon or nitrogen.
Wherein the flow rate of the specific atmosphere is 0-160 ml/min, preferably 30-80 ml/min.
Wherein the annealing temperature is 300-900 ℃, preferably 450-700 ℃.
Wherein the temperature rise rate of the annealing treatment is 3-10 ℃/min, and the high-temperature holding time is 30-300 min, preferably 30-100 min.
Wherein, the separation capability of electron-hole is improved by changing VO x -Ga 2 O 3 The open circuit voltage and the valence band energy level difference of the heterojunction photoelectric device are realized. The invention can make VO through secondary specific atmosphere annealing x -Ga 2 O 3 The open-circuit voltage of the heterojunction photoelectric device is increased to 0.3-1.2V, so that VO is generated x -Ga 2 O 3 The absolute value of the valence band energy level difference of the heterojunction is reduced to 0.01-0.5 eV.
Wherein, the transport capability of the current carrier is improved by enhancing VO x Hole mobility of material and Ga 2 O 3 Electron mobility of the material. VO is obtained after secondary specific atmosphere annealing x The hole mobility of the material is increased to 10-3000 cm 2 /Vs，Ga 2 O 3 The electron mobility of the material is increased to 0.1-100 cm 2 /Vs。
Wherein, VO is formed by the annealing method of the present invention x The composition of the material may be varied, the valence of the element V being essentially V 5+ And V 4+ ，V 4+ /V 5+ The ratio of (A) to (B) is usually 0.1 to 10, and VO is obtained after the secondary specific atmosphere annealing x V in the material 4+ /V 5+ The ratio of (b) may be 0.3 to 1.5.
The invention also discloses a VO x -Ga 2 O 3 The preparation method of the heterojunction comprises the following steps：
Preparation of VO x -Ga 2 O 3 A heterojunction;
for prepared VO x -Ga 2 O 3 And carrying out secondary specific atmosphere annealing on the heterojunction to improve the separation capability of electron-hole and the carrier transport capability.
Wherein the prepared VO x -Ga 2 O 3 The heterojunction is one of a planar heterojunction and a vertical heterojunction, wherein Ga 2 O 3 Is a film with the thickness of 50-900 nm, VO x Is a thin film with the thickness of 5-200 nm.
Wherein the specific atmosphere is formed by one or more of air, oxygen, argon and nitrogen.
Wherein the flow rate of the specific atmosphere is 0-160 ml/min, preferably 30-80 ml/min.
Wherein the annealing temperature is 300-900 ℃, preferably 450-700 ℃.
Wherein the temperature rise rate of the annealing treatment is 3-10 ℃/min, and the high-temperature holding time is 30-300 min, preferably 30-100 min.
The invention also discloses VO prepared by the preparation method x -Ga 2 O 3 A heterojunction.
Wherein, the VO x -Ga 2 O 3 In the heterojunction, VO x The hole mobility of the material is increased to 10-3000 cm 2 /Vs，Ga 2 O 3 The electron mobility of the material is increased to 0.1-100 cm 2 /Vs。
The invention also discloses a photoelectric device, wherein the photoelectric device comprises the VO x -Ga 2 O 3 A heterojunction.
Wherein the open-circuit voltage of the photoelectric device is increased to 0.3-1.2V, and the absolute value of the valence band energy level difference is reduced to 0.01-0.5 eV.
Wherein the photoelectric device is a self-powered photoelectric detector.
In order that the objects, technical solutions and advantages of the present invention will become more apparent, the present invention will be further described in detail with reference to the accompanying drawings in conjunction with the following specific embodiments. It should be noted that the following examples are only for illustrating the present invention and are not intended to limit the present invention.
Unless otherwise specified, the means mentioned in the examples are conventional in the art.
Example 1
Al in (0001) orientation by metalorganic chemical vapor deposition 2 O 3 Preparation of Ga on a substrate 2 O 3 A film. Precursor solution prepared from triisopropoxytriantiovanadium oxide and isopropanol in Ga 2 O 3 And spin coating the film to prepare a precursor layer. Ga prepared preliminarily 2 O 3 /VO x Annealing the precursor layer on a hot platform for 10min at 100 ℃ in natural air to obtain VO x -Ga 2 O 3 A thin film heterojunction (1). To realize VO x -Ga 2 O 3 Improvement of heterojunction photoresponse performance to the primarily obtained VO x -Ga 2 O 3 Carrying out secondary annealing on the thin film heterojunction (1) in a specific atmosphere, wherein the annealing atmosphere is argon, the flow rate of the annealing atmosphere is 40ml/min, the annealing temperature is 500 ℃, and the annealing time is 60min to obtain VO x -Ga 2 O 3 A thin film heterojunction (2).
VO respectively given to heterojunction by magnetron sputtering method x And Ga 2 O 3 Preparing Ti/Au electrode with thin film to form ohmic contact, and preparing VO-based x -Ga 2 O 3 A heterojunction photovoltaic device.
VO-based x -Ga 2 O 3 The annealing condition of the photoelectric device prepared by the thin film heterojunction (1) is 100 ℃ in an air atmosphere, and the obtained dark current and photocurrent are shown in figure 1. Under the condition of light with the wavelength of 254nm and the illumination intensity of 1mW/cm 2 Under the bias of-5V, the obtained dark current is 0.3pA, and the photocurrent is 37.6nA. At the same time, VO prepared initially x -Ga 2 O 3 The film heterojunction (1) has self-power supply capacity, and the open-circuit voltage under illumination is 0.4V and 0V under bias voltageThe optical response is realized, and the optical response curve along with the switching of the optical switch is shown in figure 2. 0V bias, 1mW/cm 2 The current under illumination with a wavelength of 254nm was 3.7nA.
VO based on secondary argon annealing x -Ga 2 O 3 The annealing condition of the photoelectric device prepared by the thin film heterojunction (2) is 500 ℃ in an argon atmosphere, and the obtained dark current and photocurrent are shown in figure 1. Under the condition of light with the wavelength of 254nm and the illumination intensity of 1mW/cm 2 Under the bias of-5V, the obtained dark current is 0.4pA, and the photocurrent is 1497.6nA. At the same time, VO after secondary annealing x -Ga 2 O 3 The thin film heterojunction (2) has self-power supply capability, and can realize optical response under the bias of 0.66V and 0V, and the optical response curve along with the switching of the optical switch is shown in FIG. 2. 0V bias, 1mW/cm 2 The current under illumination with a wavelength of 254nm is 209nA.
Compared with the VO prepared initially, the performance of the photoelectric test shows that x -Ga 2 O 3 The heterojunction photoelectric device is subjected to annealing in a specific atmosphere, the dark current of the photoelectric device is almost unchanged, the photocurrent is improved by 39.8 times, the open-circuit voltage of the photoelectric device is increased from 0.4V to 0.66V, and the self-supply current is improved by 56.5 times.
Initial preparation and secondary annealing treatment VO x -Ga 2 O 3 The spectral response curve of the heterojunction photoelectric device under 0V bias is shown in figure 3, and VO is obtained by annealing twice with argon gas x -Ga 2 O 3 The photoresponse performance of the heterojunction photoelectric device is greatly improved.
Second specific atmosphere annealing of VO x -Ga 2 O 3 The improvement of the self-powered performance of the heterojunction photoelectric device is obtained based on the optimization of a heterojunction self-powered working mechanism. By changing the contact characteristic at the interface and improving the conductivity of the heterojunction composition material, the separation efficiency of electron-hole pairs and the transport capacity of carriers are improved, and the working efficiency of the device is improved.
The enhanced electron-hole separation capability is illustrated by an increase in open circuit voltage, which indicates an increase in the separation pulling force of the exciton states at the interface.
The improvement of the carrier transport capability can be explained by the carrier mobility of the material. Wherein, VO x The hole conductivity of the material is improved as shown in FIG. 4, VO is at-5V bias during initial preparation x The dark current of the film was 32nA; VO under-5V bias after secondary annealing x The dark current of the film is 15554.3nA, and the hole mobility is as high as about 2000cm 2 and/Vs, the hole transport capacity is improved by 486 times.
VO-based x -Ga 2 O 3 The measured interface level alignment of the thin film heterojunction (1) is shown in FIG. 5, ga 2 O 3 Valence band and VO x Energy level difference of valence band is Delta E V ＝0.62eV。
VO-based x -Ga 2 O 3 Alignment chart of measured interface level of thin film heterojunction (2), as shown in FIG. 6, ga 2 O 3 Valence band and VO x Energy level difference of valence band is Delta E V ＝0.12eV。
The reduction of the valence band energy level difference at the heterojunction interface is more beneficial to the transition migration of holes, and the separation efficiency of electrons and holes and the transport speed of carriers are improved.
Examples 2 to 4
The specific experimental method is different from that of example 1 only in the setting of the annealing atmosphere, the annealing temperature and the like, and the differences of the specific experimental parameters and the performance indexes are detailed in the following table 1.
Comparative example
The specific test parameters and device performance indicators for the comparative examples were derived from the VO in example 1 x -Ga 2 O 3 Thin film heterojunction (1), the only difference being that the comparative example only carries out the first annealing. The differences between the specific test parameters and performance criteria are detailed in table 1 below, wherein it is noted that the air and 100 ℃ of comparative example 1 in table 1 refer to the annealing atmosphere and annealing temperature, respectively, at the first annealing, and the annealing atmosphere and annealing temperature in examples 1-4 refer to the annealing atmosphere and annealing temperature, respectively, at the second annealing.
TABLE 1 detailed comparison of specific test parameters and Performance indices for examples 1-4 and comparative examples
Note: open circuit voltage is 1mW/cm of illumination intensity 2 Measured under 254nm light; VO (vacuum vapor volume) x Dark current value is measured under-5V bias voltage; the self-supply current is VO x -Ga 2 O 3 When the heterojunction photoelectric detector is biased at 0V, the illumination intensity is 1mW/cm 2 Measured under 254nm light; VO (vacuum vapor volume) x -Ga 2 O 3 The spectral electrical responsivity of the heterojunction photodetector was measured by a xenon lamp spectrometer and is listed in the table as the 0V bias responsivity at a wavelength of 245 nm.
Based on the demonstration of the above embodiment, it can be proved that the method of the present invention enhances the separation of electron-hole and the transport of photo-generated carriers from the working mechanism of the heterojunction photoelectric device by annealing in a specific atmosphere, and effectively realizes VO x -Ga 2 O 3 Enhancement of heterojunction self-powered photoresponse performance.
While the foregoing embodiments have described the objects, aspects and advantages of the present invention in further detail, it should be understood that the present invention is not inherently related to any particular computer, virtual machine or electronic device, and various general-purpose machines may be used to implement the present invention. The invention is not to be considered as limited to the specific embodiments thereof, but is to be understood as being modified in all respects, all changes and equivalents that come within the spirit and scope of the invention.
Claims (12)
1. Enhanced VO x -Ga 2 O 3 A method of heterojunction self-powered photo-responsive performance, comprising the steps of:
initial preparation of VO x -Ga 2 O 3 A heterojunction comprising a first annealing step;
for VO obtained by initial preparation x -Ga 2 O 3 The heterojunction is subjected to second specificationAtmosphere annealing to improve the electron-hole separation capability and the carrier transport capability; wherein the specific atmosphere of the second specific atmosphere annealing is an atmosphere formed by one or a combination of more of air, oxygen, argon and nitrogen, and the annealing temperature of the second specific atmosphere annealing is 300-900 ℃.
2. The method of claim 1, wherein the VO is prepared x -Ga 2 O 3 The heterojunction is one of a planar heterojunction and a vertical heterojunction, wherein Ga 2 O 3 Is a film with the thickness of 50-900 nm, VO x Is a thin film with the thickness of 5-200 nm.
3. The method according to claim 2, wherein the flow rate of the specific atmosphere is 0 to 160ml/min, excluding 0ml/min; and/or
The annealing temperature is 450-700 ℃; and/or
The temperature rising speed of the second specific atmosphere annealing is 3-10 ℃/min, and the high-temperature holding time is 30-300 min.
4. The method according to claim 3, wherein the flow rate of the specific atmosphere is 30 to 80ml/min; and/or
The high-temperature holding time is 30-100 min.
5. VO (volatile organic compound) x -Ga 2 O 3 The preparation method of the heterojunction is characterized by comprising the following steps:
initial preparation of VO x -Ga 2 O 3 A heterojunction comprising a first annealing step;
for the initially prepared VO x -Ga 2 O 3 Carrying out secondary specific atmosphere annealing on the heterojunction to improve the separation capability of electron-hole and the carrier transport capability; wherein, the specific atmosphere of the second specific atmosphere annealing is an atmosphere formed by one or more of air, oxygen, argon and nitrogen in combination, and the second specific atmosphere annealing is carried outThe annealing temperature of the secondary specific atmosphere annealing is 300-900 ℃.
6. The method of claim 5, wherein the VO is prepared x -Ga 2 O 3 The heterojunction is one of a planar heterojunction and a vertical heterojunction, wherein Ga 2 O 3 Is a film with the thickness of 50-900 nm, VO x Is a thin film with the thickness of 5-200 nm.
7. The method according to claim 6, wherein the flow rate of the specific atmosphere is 0 to 160ml/min, excluding 0ml/min; and/or
The annealing temperature is 450-700 ℃; and/or
The temperature rising speed of the second specific atmosphere annealing is 3-10 ℃/min, and the high-temperature holding time is 30-300 min.
8. The method according to claim 7, wherein the flow rate of the specific atmosphere is 30 to 80ml/min; and/or
The high-temperature holding time is 30-100 min.
9. VO prepared by the preparation method according to any one of claims 5 to 8 x -Ga 2 O 3 A heterojunction.
10. The VO of claim 9 x -Ga 2 O 3 A heterojunction characterized by said VO x -Ga 2 O 3 In the heterojunction, VO x The hole mobility of the material is increased to 10-3000 cm 2 /Vs，Ga 2 O 3 The electron mobility of the material is increased to 0.1-100 cm 2 /Vs。
11. An optoelectronic device comprising a VO according to claim 9 or 10 therein x -Ga 2 O 3 A heterojunction.
12. The optoelectronic device according to claim 11, wherein the open circuit voltage of the optoelectronic device increases from 0.3 to 1.2V, and the absolute value of the valence band energy level difference decreases from 0.01 to 0.5eV; and/or
The photoelectric device is a self-powered photoelectric detector.
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